Mesoscale Multi-Shell Architectures with DNA-Programmable Nanoscale Organization

DNA-based assembly approaches offer the creation of highly ordered and functional nanomaterials by leveraging the programmability of DNA sequences. This approach enables precise spatial control, allowing the assembly of complex structures through engineered bonds to program the placement of functional nanoparticles. However, to fully utilize these new materials for applications in optics, energy materials, and biomaterials, it is required to develop methods for controlling multiple scales, from nano- to meso- and macro-regimes. <br/>To address this challenge, we have explored the creation of multi-shell DNA-based lattice architectures with both nanoscale and mesoscale organization. We developed an epitaxial growth strategy for fabricating multi-shell DNA superlattices by controlling DNA crystal growth via selective assembly of monomers. This approach leverages the designed binding capabilities of DNA scaffold, enabling precise formation and in-situ monitoring of shell growth. The developed methodology overcomes nucleation challenges, facilitating the creation of complex multi-shell DNA superlattices. We used the developed approach to control nanoparticle loading and release within the mesoscale structure and analyzed the kinetics of these processes. Our investigation demonstrates the effectiveness of multi-shell DNA superlattices as carriers for controlled release applications, offering promising avenues for enhanced stability and efficacy in drug delivery systems. Additionally, through the design of directional bonds of monomers and control of assembly processes, we further demonstrate that this strategy allows for the creation of intricate configurations such as Janus-like and dumbbell mesoscale architectures.